Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine

Erik P. Mansson, Simone Latini, Fabio Covita, Vincent Wanie, Mara Galli, Enrico Perfetto, Gianluca Stefanucci, Hannes Hübener, Umberto De Giovannini, Mattea C. Castrovilli, Andrea Trabattoni, Fabio Frassetto, Luca Poletto, Jason B. Greenwood, François Légaré, Mauro Nisoli, Angel Rubio, Francesca Calegari

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Abstract

Sudden ionisation of a relatively large molecule can initiate a correlation-driven process dubbed charge migration, where the electron density distribution is expected to rapidly move along the molecular backbone. Capturing this few-femtosecond or attosecond charge redistribution would represent the real-time observation of electron correlation in a molecule with the enticing prospect of following the energy flow from a single excited electron to the other coupled electrons in the system. Here, we report a time-resolved study of the correlation-driven charge migration process occurring in the nucleic-acid base adenine after ionisation with a 15–35 eV attosecond pulse. We find that the production of intact doubly charged adenine – via a shortly-delayed laser-induced second ionisation event – represents the signature of a charge inflation mechanism resulting from many-body excitation. This conclusion is supported by first-principles time-dependent simulations. These findings may contribute to the control of molecular reactivity at the electronic, few-femtosecond time scale.
Original languageEnglish
Article number73
Number of pages7
JournalCommunications Chemistry
Volume4
DOIs
Publication statusPublished - 20 May 2021

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